Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 28, Pages 9640-9645Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201905241
Keywords
adsorption energy; fuel cells; iridium; oxygen reduction reaction; single-atom catalyst
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Funding
- University of Waterloo
- Wenzhou University
- Automotive Partnership Canada (APC) Grant through the Natural Sciences and Engineering Research Council of Canada (NSERC) [APCPJ 417858-11]
- National Natural Science Foundation of China [51872209, 51772219]
- Zhejiang Provincial Natural Science Foundation of China [LZ17E02002]
- U.S. Department of Energy (DOE), Office of Basic Energy Science [DE-SC0012704]
- U.S. Department of Energy (DOE) Office of Science [DE-AC02-06CH11357]
- U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office
- DOE Office of Science [DE-AC02-06CH11357]
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Combining the advantages of homogeneous and heterogeneous catalysts, single-atom catalysts (SACs) are bringing new opportunities to revolutionize ORR catalysis in terms of cost, activity and durability. However, the lack of high-performance SACs as well as the fundamental understanding of their unique catalytic mechanisms call for serious advances in this field. Herein, for the first time, we develop an Ir-N-C single-atom catalyst (Ir-SAC) which mimics homogeneous iridium porphyrins for high-efficiency ORR catalysis. In accordance with theoretical predictions, the as-developed Ir-SAC exhibits orders of magnitude higher ORR activity than iridium nanoparticles with a record-high turnover frequency (TOF) of 24.3e(-) site(-1)s(-1) at 0.85V vs. RHE) and an impressive mass activity of 12.2Amg(Ir)(-1), which far outperforms the previously reported SACs and commercial Pt/C. Atomic structural characterizations and density functional theory calculations reveal that the high activity of Ir-SAC is attributed to the moderate adsorption energy of reaction intermediates on the mononuclear iridium ion coordinated with four nitrogen atom sites.
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